IP Library Granted Patent US 11,814,285
Granted Patent B2
US 11,814,285 · App. 16/764,226 · Granted Nov 14, 2023

Simultaneous reaction and separation of chemicals

Inventors: Eric W. McFarland (Santa Barbara, CA); Ches Upham (Menlo Park, CA); Jiren Zeng (Goleta, CA); Clarke Palmer (Goleta, CA); Shizhao Su (Santa Barbara, CA); Davide Mannini (Santa Barbara, CA); Dohyung Kang (Goleta, CA); Nazanin Rahimi (Goleta, CA); Horia Metiu (Santa Barbara, CA); Michael Gordon (Goleta, CA)
Assignee: THE REGENTS OF THE UNIVERSITY OF CALIFORNIA
C01B3/26B01J8/0278B01J23/825B01J23/8437B01J27/08B01J35/0006B01J35/12C01B2203/0277C01B2203/1011C01B2203/1058C01B2203/1241
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Quick Facts
Patent No.
US 11,814,285
App. No.
16/764,226
Granted
Nov 14, 2023
Kind
B2
Abstract

The reaction rate of hydrocarbon pyrolysis can be increased to produce solid carbon and hydrogen by the use of molten materials which have catalytic functionality to increase the rate of reaction and physical properties that facilitate the formation and contamination-free separation of the solid carbon. Processes, materials, reactor configurations, and conditions are disclosed whereby methane and other hydrocarbons can be decomposed at high reaction rates into hydrogen gas and carbon products without any carbon oxides in a single reaction step. The process also makes use of specific properties of selected materials with unique solubilities and/or wettability of products into (and/or by) the molten phase to facilitate generation of purified products and increased conversion in more general reactions.

Claims (32)

1. A multiphase reaction system comprising:

a reactor vessel, the reactor vessel comprising:

a feed stream comprising one or more hydrocarbon gas phase reactants;

liquid phases comprising a first liquid and a second liquid, the first liquid comprising a molten metal or a metalloid, and the second liquid comprising a molten salt, wherein the molten salt is disposed as a separate phase on top of the molten metal or the metalloid;

a solid phase disposed within the liquid phases; and

one or more products, wherein the one or more products comprise solid carbon and hydrogen, wherein the solid phase and the solid carbon are different, and wherein the solid carbon is accumulated on top of the molten salt.

2. The multiphase reaction system of claim 1 , wherein the solid phase comprises a solid phase catalyst.

3. The multiphase reaction system of claim 1 , wherein the solid phase is assembled as a packed bed of solid particles or pellets with the liquid phases between the solid particles or the pellets, and wherein the solid particles or the pellets have catalytic activity to the one or more gas phase reactants.

4. The multiphase reaction system of claim 1 , wherein the solid phase comprises a metal, wherein the metal comprises nickel, iron, cobalt, copper, platinum, ruthenium, rhodium, or any combination thereof.

5. The multiphase reaction system of claim 1 , wherein the solid phase comprises a mixed metal oxide, wherein the mixed metal oxide comprises titanium oxide, zirconia, tungsten oxide, or any combination thereof.

6. The multiphase reaction system of claim 5 , wherein the solid phase is supported on alumina, silica, zirconia, or any combination thereof.

7. The multiphase reaction system of claim 1 , wherein the molten salt comprises NaCl, NaBr, KCl, KBr, LiCl, LiBr, CaCl 2 , MgCl 2 , CaBr 2 , MgBr 2 , or any combination thereof.

8. The multiphase reaction system of claim 1 , further comprising:

a gas inlet configured to introduce a gas stream into the reactor vessel above the liquid phases; entrain at least a portion of the solid carbon in the gas stream; and

remove the portion of the solid carbon from the reactor vessel in the gas stream.

9. The multiphase reaction system of claim 1 , wherein the molten metal comprises Ni, Co, Fe, Pd, Cu, Pt, Al, Sn, Pb, Au, Ag, In, Ga, Te, Bi, Sb, or any mixture thereof.

10. The system of claim 1 , wherein the molten metal or the metalloid has catalytic properties towards a reaction of the one or more hydrocarbon gas phase reactants.

11. The system of claim 1 , wherein the molten salt has a lower density than that of the molten metal or the metalloid.

12. A multiphase reaction method, the method comprising:

contacting one or more gas phase reactants with a solid phase disposed within liquid phases in a reactor, wherein the liquid phases comprises a first liquid and a second liquid, wherein the first liquid comprises a molten metal or a metalloid, wherein the second liquid comprises a molten salt, wherein the molten salt is disposed as a separate phase on top of the molten metal or the metalloid, wherein the one or more gas phase reactants comprise a hydrocarbon, and wherein the solid phase comprises a solid phase catalyst; and

producing one or more reaction products in response to contacting the one or more gas phase reactants with the solid phase, wherein the one or more reaction products comprise solid carbon and hydrogen, and wherein the solid carbon is accumulated on top of the molten salt.

13. The method of claim 12 , further comprising:

solvating or removing at least a portion of the one or more reaction products on the solid phase with the liquid phases, wherein the one or more reaction products solvated or removed with the liquid phases comprise at least a portion of the solid carbon; and

separating at least the portion of the one or more reaction products from the one or more gas phase reactants in response to the solvating or the removing.

14. The method of claim 12 , wherein the solid phase is assembled as a packed bed of solid particles or pellets with the liquid phase between the solid particles or the pellets, and wherein the solid particles or the pellets have catalytic activity to the one or more gas phase reactants.

15. The method of claim 12 , wherein the solid phase comprises a metal, wherein the metal comprises nickel, iron, cobalt, copper, platinum, ruthenium, rhodium, or any combination thereof.

16. The method of claim 15 , wherein the solid phase is supported on alumina, silica, zirconia, or any combination thereof.

17. The method of claim 12 , wherein the solid phase comprises a mixed metal oxide, wherein the mixed metal oxide comprises titanium oxide, zirconia, tungsten oxide, or any combination thereof.

18. The method of claim 12 , wherein the molten salt comprises NaCl, NaBr, KCl, KBr, LiCl, LiBr, CaCl 2 , MgCl 2 , CaBr 2 , MgBr 2 , or any combination thereof.

19. The multiphase reaction method of claim 12 , wherein the molten metal comprises Ni, Co, Fe, Pd, Cu, Pt, Al, Sn, Pb, Au, Ag, In, Ga, Te, Bi, Sb, or any mixture thereof.

20. The multiphase method of claim 12 , wherein the molten metal or the metalloid has catalytic properties towards a reaction of the one or more hydrocarbon gas phase reactants.

21. The method of claim 12 , wherein the molten salt has a lower density than that of the molten metal or the metalloid.

Assignments (2)
CONFIRMATORY LICENSE Recorded Oct 22, 2020
From: UNIVERSITY OF CALIFORNIA SANTA BARBARA
To: UNITED STATES DEPARTMENT OF ENERGY
Reel/Frame 054175/0788 →
ASSIGNMENT OF ASSIGNOR'S INTEREST Recorded May 14, 2020
From: MCFARLAND, ERIC W.; UPHAM, CHES; ZENG, JIREN; PALMER, CLARKE; SU, SHIZHAO; MANNINI, DAVIDE; KANG, DOHYUNG; RAHIMI, NAZANIN; METIU, HORIA; GORDON, MICHAEL
To: THE REGENTS OF THE UNIVERSITY OF CALIFORNIA
Reel/Frame 052666/0946 →
Continuity (2)
Provisional Application 62586943 · Nov 16, 2017
Related Publication 20200283293A1 · Sep 10, 2020